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The origin of the pseudogap in many strongly correlated materials has been a longstanding puzzle. Here, we present experimental evidence that many-body interactions among small Holstein polarons, i.e., the formation of bipolarons, are primarily responsible for the pseudogap in (TaSe4)2I. After weak photoexcitation of the material, we observe the appearance of both dispersive (single-particle bare band) and flat bands (single-polaron sub-bands) in the gap by using time- and angle-resolved photoemission spectroscopy. Based on Monte Carlo simulations of the Holstein model, we propose that the melting of pseudogap and emergence of new bands originate from a bipolaron to single-polaron crossover. We also observe dramatically different relaxation times for the excited in-gap states in (TaSe4)2I (∼600 fs) compared with another 1D material Rb0.3MoO3(∼60 fs), which provides a new method for distinguishing between pseudogaps induced by polaronic or Luttinger-liquid many-body interactions.

A long-standing open problem in condensed-matter physics is whether or not a strongly disordered interacting insulator can be mapped to a system of effectively non-interacting localized excitations. Using terahertz two-dimensional coherent spectroscopy, we investigate this issue in phosphorus-doped silicon, a classic example of a correlated disordered electron system in three dimensions. Despite the intrinsically disordered nature of these materials, we observe coherent excitations and strong photon echoes that provide us with a powerful method for the study of their decay processes. We extract the energy relaxation and decoherence rates close to the metal–insulator transition. We observe that both rates are linear in excitation frequency with a slope close to unity. The energy relaxation timescale counterintuitively increases with increasing temperature, and the coherence relaxation timescale has little temperature dependence below 25 K, but increases as the material is doped towards the metal–insulator transition. Here we argue that these features imply that the system behaves as a well-isolated electronic system on the timescales of interest, and relaxation is controlled by electron–electron interactions. Our observations constitute a distinct phenomenology, driven by the interplay of strong disorder and strong electron–electron interactions, which we dub the marginal Fermi glass.